Algorithms are presented which were created and implemented by the Goddard Space Flight Center's (GSFC's) Solar Maximum Mission (SMM) attitude operations team to support large-angle spacecraft pointing at scientific objectives. The mission objective of the post-repair SMM satellite was to study solar phenomena. However, because the scientific instruments, such as the Coronagraph/Polarimeter (CP) and the Hard X ray Burst Spectrometer (HXRBS), were able to view objects other than the Sun, attitude operations support for attitude pointing at large angles from the nominal solar-pointing attitudes was required. Subsequently, attitude support for SMM was provided for scientific objectives such as Comet Halley, Supernova 1987A, Cygnus X-1, and the Crab Nebula. In addition, the analysis was extended to include the reverse problem, computing the right ascension and declination of a body given the off-Sun angles. This analysis led to the computation of the orbits of seven new solar comets seen in the field-of-view (FOV) of the CP. The activities necessary to meet these large-angle attitude-pointing sequences, such as slew sequence planning, viewing-period prediction, and tracking-bias computation are described. Analysis is presented for the computation of maneuvers and pointing parameters relative to the SMM-unique, Sun-centered reference frame. Finally, science data and independent attitude solutions are used to evaluate the large-angle pointing performance.